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Density Functional Tight Binding (DFTB) is an attractive method for accelerated quantum simulations of condensed matter due to its enhanced computational efficiency over standard Density Functional Theory approaches. However, DFTB models…

Density-functional based tight-binding is a powerful method to describe large molecules and materials. Metal-Organic Frameworks (MOFs), materials with interesting catalytic properties and with very large surface areas have been developed…

A precise understanding of mechanisms governing the dynamics of electrons in atoms and molecules subjected to intense laser fields has a key importance for the description of attosecond processes such as the high-harmonic generation and…

We demonstrate that basis sets suitable for electronic structure calculations can be obtained from simple accuracy considerations for the hydrogenic one-electron ions $Y^{(Y-1)+}$ for $Y\in[1,Z]$, necessitating no self-consistent field…

Computational Physics · Physics 2020-04-06 Susi Lehtola

Gausslets are one of the few basis constructions for electronic structure that combine locality, orthonormality, variable resolution, and an accurate diagonal approximation for the electron-electron interaction, but the original…

Chemical Physics · Physics 2026-05-07 Steven R. White

We present the implementation of a variational finite element solver in the HelFEM program for benchmark calculations on diatomic systems. A basis set of the form $\chi_{nlm}(\mu,\nu,\phi)=B_{n}(\mu)Y_{l}^{m}(\nu,\phi)$ is used, where…

Chemical Physics · Physics 2019-08-19 Susi Lehtola

The perovskite oxides are known to be susceptible to structural distortions over a long wavelength when compared to their parent cubic structures. From an ab initio simulation perspective, this requires accurate calculations including many…

Computational Physics · Physics 2022-02-16 Jack S. Baker , Tsuyoshi Miyazki , David R. Bowler

This article is a pedagogical introduction to density-functional tight-binding (DFTB) method. We derive it from the density-functional theory, give the details behind the tight-binding formalism, and give practical recipes for…

Materials Science · Physics 2009-11-02 Pekka Koskinen , Ville Mäkinen

Density functional calculations on atoms are often used for determining accurate initial guesses as well as generating various types of pseudopotential approximations and efficient atomic-orbital basis sets for polyatomic calculations. To…

Computational Physics · Physics 2023-10-30 Susi Lehtola

We report a universal density-based basis-set incompleteness correction that can be applied to any wave function method. The present correction, which appropriately vanishes in the complete basis set (CBS) limit, relies on short-range…

We introduce a mixed density fitting scheme that uses both a Gaussian and a plane-wave fitting basis to accurately evaluate electron repulsion integrals in crystalline systems. We use this scheme to enable efficient all-electron Gaussian…

Chemical Physics · Physics 2017-11-22 Qiming Sun , Timothy C. Berkelbach , James D. McClain , Garnet Kin-Lic Chan

To explore the applicability of orbital-free density functional theory (OF-DFT) in nuclear physics, we perform a systematic benchmark of 36 one-point kinetic energy density functionals, which are originally developed for electron systems in…

Nuclear Theory · Physics 2026-05-20 Tian Shuai Shang , Jian Li , Haozhao Liang , Xinhui Wu , Cheng Ma , Wenhui Mi , Xuecheng Shao , Yanchao Wang

Constructing a classical potential suited to simulate a given atomic system is a remarkably difficult task. This chapter presents a framework under which this problem can be tackled, based on the Bayesian construction of nonparametric force…

Computational Physics · Physics 2020-07-01 Aldo Glielmo , Claudio Zeni , Ádám Fekete , Alessandro De Vita

Large atomic-orbital (AO) basis sets of at least triple and preferably quadruple-zeta (QZ) size are required to adequately converge Kohn-Sham density functional theory (DFT) calculations towards the complete basis set limit. However,…

Chemical Physics · Physics 2025-12-02 Anthony O. Lara , Justin J. Talbot , Zhe Wang , Martin Head-Gordon

The task of deducing three-dimensional molecular configurations from their two-dimensional graph representations holds paramount importance in the fields of computational chemistry and pharmaceutical development. The rapid advancement of…

Biomolecules · Quantitative Biology 2025-01-09 Bobin Yang , Jie Deng , Zhenghan Chen , Ruoxue Wu

Double-hybrid density functional theory (DHDFT) offers a pathway to accuracies approaching composite wavefunction approaches like G4 theory. However, the GLPT2 (G{\"o}rling 2nd order perturbation theory) term causes them to partially…

Chemical Physics · Physics 2022-10-13 Nisha Mehta , Jan M. L. Martin

We present a new efficient way to perform hybrid density functional theory (DFT) based electronic structure calculation. The new method uses an interpolative separable density fitting (ISDF) procedure to construct a set of numerical…

Computational Physics · Physics 2017-07-31 Wei Hu , Lin Lin , Chao Yang

We report an efficient algorithm using density fitting for the relativistic complete active space self-consistent field (CASSCF) method, which is significantly more stable than the algorithm previously reported by one of the authors [J. E.…

Chemical Physics · Physics 2018-08-01 Ryan D. Reynolds , Takeshi Yanai , Toru Shiozaki

In this article we present an algorithm to efficiently evaluate the exchange matrix in periodic systems when Gaussian basis set with pseudopotentials are used. The usual algorithm for evaluating exchange matrix scales cubically with the…

Strongly Correlated Electrons · Physics 2022-11-11 Sandeep Sharma , Alec F. White , Gregory Beylkin

A linear-scaling algorithm is presented for computing the Hartree-Fock (HF) exchange matrix using concentric atomic density fitting. The algorithm utilizes the stronger distance dependence of the three-center electron repulsion integrals…

Chemical Physics · Physics 2014-10-21 David S. Hollman , Henry F. Schaefer , Edward F. Valeev